The present invention relates to (2,5-disubstituted-1,4-phenylene oxide) copolymers.
Poly (2,6-disubstituted-1,4-phenylene oxide) is synthesized by oxidative polymerization of 2,6-disubstituted phenols, and it is widely known to show high heat resistance. For example, poly (2,6-dimethyl-1,4-phenylene oxide) is reported in J. Am. Chem. Soc., 81, 6335-6336 (1959), and poly (2,6-diphenyl-1,4-phenylene oxide) is reported in Macromolecules, 2, 107-108 (1969). Phenols with substituents at positions 2 and 6 are used in order to block coupling of the two ortho positions, as described in J. Polym. Sci.: Part A: Polymer Chemistry, 36, 505-517 (1998).
The inventors succeeded in synthesizing crystalline poly (2,5-dimethyl-1,4-phenylene oxide) from 2,5-dimethylphenol, which does not have a substituent at one ortho position (see Japanese Patent Application No. 2000-25621). The polymer shows a high crystalline melting point, even after melting and cooling, and it is expected to be a crystalline polymer having high heat resistance and solvent resistance. However, the mechanical properties and impact strength of molded articles made from this polymer have not been satisfactory enough, therefore further improvement is needed.
The present invention is a (2,5-disubstituted-1,4-phenylene oxide) block copolymer which comprises one or more block structural units represented by the following formula (I) and at least one structural unit represented by the following formula (II) or the following formula (III) in a molecule, 
wherein R1 represents an unsubstituted hydrocarbon group or a substituted hydrocarbon group, and the two R1s may be the same or different; R2 represents an unsubstituted arylene group or a substituted arylene group; R3 represents an unsubstituted alkylene group, a substituted alkylene group, an unsubstituted alkylene group, a substituted aralkylene group, an unsubstituted alkenylene group, a substituted alkenylene group, an unsubstituted aralkenylene group, a substituted aralkenylene group, an unsubstituted alkynylene group, a substituted alkynylene group, an unsubstituted aralkynylene group, or a substituted aralkynylene group; T represents xe2x80x94COxe2x80x94, xe2x80x94CONHxe2x80x94 or xe2x80x94SO2xe2x80x94; Q represents xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94SO2xe2x80x94, xe2x80x94OCOxe2x80x94, xe2x80x94NHCOxe2x80x94, or xe2x80x94OSi(CH3)2xe2x80x94; a represents a number average degree of polymerization and is the number of 5 or more; and b, c, d, and e are each 1 or 0, and at least one of c, d, or e is 1.
Further the present invention is a (2,5-disubstituted-1,4-phenylene oxide) graft polymer which comprises one or more structural units represented by the following formula (IV), or three or more of structural unit of the following formula (IV) and structural unit of the following formula (V), in a molecule, 
wherein R1 represents an unsubstituted hydrocarbon group or a substituted hydrocarbon group, and the two R1s may be the same or different; R4 and R5 each represents a trifunctional unsubstituted hydrocarbon group or a trifunctional substituted hydrocarbon group; R6 represents a hydrogen atom, a halogen atom, an unsubstituted hydrocarbon group, or a substituted hydrocarbon group; U represents xe2x80x94COxe2x80x94, xe2x80x94OCOxe2x80x94, or xe2x80x94NHCOxe2x80x94; W represents xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94CO2xe2x80x94 xe2x80x94OCOxe2x80x94, or xe2x80x94CONHxe2x80x94; a represents a number average degree of polymerization and is the number of 5 or more; and f and g are each 1 or 0.
Other and further features, and advantages of the invention will appear more fully from the following description.
According to the present invention, there is provided:
(1) A (2,5-disubstituted-1,4-phenylene oxide) block copolymer which comprises one or more block structural units represented by the following formula (I) and at least one structural unit represented by the following formula (II) or the following formula (III) in a molecule, 
wherein R1 represents an unsubstituted hydrocarbon group or a substituted hydrocarbon group, and the two R1s may be the same or different; R2 represents an unsubstituted arylene group or a substituted arylene group; R3 represents an unsubstituted alkylene group, a substituted alkylene group, an unsubstituted aralkylene group, a substituted aralkylene group, an unsubstituted alkenylene group, a substituted alkenylene group, an unsubstituted aralkenylene group, a substituted aralkenylene group, an unsubstituted alkynylene group, a substituted alkynylene group, an unsubstituted aralkynylene group, or a substituted aralkynylene group; T represents xe2x80x94COxe2x80x94, xe2x80x94CONHxe2x80x94 or xe2x80x94SO2xe2x80x94; Q represents xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94SO2xe2x80x94, xe2x80x94OCOxe2x80x94, xe2x80x94NHCOxe2x80x94, or xe2x80x94OSi(CH3)2xe2x80x94; a represents a number average degree of polymerization and is the number of 5 or more; and b, c, d, and e are each 1 or 0, and at least one of c, d, or e is 1;
(2) The (2,5-disubstituted-1,4-phenylene oxide) block copolymer according to (1), wherein a in the formula (I) is 5 to 5,000, and, in a molecule, the number of the block structural units represented by the formula (I) is 1 to 1,000 and the number of the structural units represented by the formula (II) and/or the formula (III) is 1 to 1,000,000;
(3) A (2,5-disubstituted-1,4-phenylene oxide) graft polymer (homopolymer or copolymer) which comprises one or more structural units represented by the following formula (IV), or three or more of structural unit of the following formula (IV) and structural unit of the following formula (V), in a molecule, 
wherein R1 represents an unsubstituted hydrocarbon group or a substituted hydrocarbon group, and the two R1s may be the same or different; R4 and R5 each represents a trifunctional unsubstituted hydrocarbon group or a trifunctional substituted hydrocarbon group; R6 represents a hydrogen atom, a halogen atom, an unsubstituted hydrocarbon group, or a substituted hydrocarbon group; U represents xe2x80x94COxe2x80x94, xe2x80x94OCOxe2x80x94, or xe2x80x94NHCOxe2x80x94; W represents xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94CO2xe2x80x94 xe2x80x94OCOxe2x80x94, or xe2x80x94CONHxe2x80x94; a represents a number average degree of polymerization and is the number of 5 or more; and f and g are each 1 or 0;
(4) The (2,5-disubstituted-1,4-phenylene oxide) graft polymer according to (3), wherein a in the formula (IV) is 5 to 5,000, and, in a molecule, the number of the structural units represented by the formula (IV) is 1 to 100,000 and the number of the structural units represented by the formula (IV) and/or the formula (V) is 3 to 1,000,000;
(5) The (2,5-disubstituted-1,4-phenylene oxide) graft polymer according to (3) or (4), wherein f in the formula (IV) is 1;
(6) The (2,5-disubstituted-1,4-phenylene oxide) block or graft polymer according to any one of (1) to (5), wherein the polymer is a powder having an average particle diameter of 5 mm or less;
(7) The (2,5-disubstituted-1,4-phenylene oxide) block or graft polymer according to any one of (1) to (6), wherein the polymer shows an exothermic peak of crystallization of 5 J/g or more at 150xc2x0 C. or more when cooled after being melted, and/or the polymer shows an endothermic peak of crystal melting of 5 J/g or more at 150xc2x0 C. or more when re-heated after the melted polymer is cooled; and
(8) The (2,5-disubstituted-1,4-phenylene oxide) block or graft polymer according to any one of (1) to (7), wherein the polymer is substantially free from gel substance.
Herein, the term xe2x80x9ca groupxe2x80x9d on a compound means to include both the group unsubstituted and the group having a further substituent thereon, unless otherwise specified.
The present invention will be described in detail hereinafter.
(1) Block Copolymer
The (2,5-disubstituted-1,4-phenylene oxide) block copolymer in the present invention means a polymer which comprises one or more block structural units represented by the above-mentioned formula (I) and one or more structural units represented by the above-mentioned formula (II) and/or the above-mentioned formula (III) in a molecule.
The unsubstituted hydrocarbon group as R1 in the above-mentioned formula (I) is preferably an alkyl group with 1 to 30 (more preferably 1 to 20) carbon atoms, an aralkyl group with 7 to 30 (more preferably 7 to 20) carbon atoms, or an aryl group with 6 to 30 (more preferably 6 to 20) carbon atoms, and the specific examples include methyl group, ethyl group, n-propyl group, iso-propyl group, n-butyl group, iso-butyl group, t-butyl group, pentyl group, cyclopentyl group, hexyl group, cyclohexyl group, octyl group, decyl group, dodecyl group, pentadecyl group, octadecyl group, benzyl group, 2-phenylethyl group, 1-phenylethyl group, phenyl group, 4-methylphenyl group, 1-naphthyl group, 2-naphthyl group, or the like.
The substituted hydrocarbon group as R1 in the above-mentioned formula (I) is preferably an alkyl group with 1 to 30 (more preferably 1 to 20) carbon atoms, an aralkyl group with 7 to 30 (more preferably 7 to 20) carbon atoms, or an aryl group with 6 to 30 (more preferably 6 to 20) carbon atoms, which is substituted with a halogen atom, an alkoxy group, a disubstituted amino group, or the like, and the specific examples include a trifluoromethyl group, a 2-t-butyloxyethyl group, a 3-diphenylaminopropyl group, or the like.
The two R1s in the above-mentioned formula (I) are preferably hydrocarbon groups with 1 to 20 carbon atoms, more preferably with 1 to 10 carbon atoms, and even more preferably 1 to 6 carbon atoms.
The symbol a in the above-mentioned formula (I) represents a number average degree of polymerization of the repeating units in the formula (I), and is the number of 5 or more. It is not preferable that the symbol a is less than 5, because the properties as a block copolymer are not fully exhibited in such a case. The symbol a is generally the number of a range from 5 to 5,000, and within this range, the number is preferably 1,000 or less, more preferably 500 or less, and even more preferably 100 or less. Within this range, the number is preferably 5 or more, more preferably 10 or more, and even more preferably 15 or more.
In the block structural units of the above-mentioned formula (I), structures other than the repeating unit (2,5-disubstituted-1,4-phenylene oxide) in the formula (I) may be included, provided that the desired properties of the block copolymer of the present invention are not impaired. Examples of the structures other than the repeating unit in the above-mentioned formula (I) include structural units represented by the following formulae (VI) to (XI), a structural unit represented by the following formula (X), a structural unit represented by the following formula (XI), or the like. The content of the structures other than the repeating unit in the above-mentioned formula (I) is preferably 20 units or less, more preferably 10 units or less, and even more preferably 5 units or less, based on 100 (2,5-disubstituted-1,4-phenylene oxide) units in the formula (I). 
(wherein R1 has the same meaning as that in the above-mentioned formula (I) and all the R1s may be the same or different) 
(wherein R7 and R8 each represents a hydrogen atom, an unsubstituted hydrocarbon group, or a substituted hydrocarbon group and the two R7s and the two R8s may be the same or different, and the two R7s and/or the two R8s may form rings) 
(wherein R7 and R8 each has the same meaning as that in the above-mentioned formula (X) and all the R7s and R8s may be the same or different, and the two R7s and/or R8s on the same benzene ring may form rings; R9 represents oxygen atom, sulfur atom, sulfonyl group, carbonyl group, a divalent unsubstituted hydrocarbon group, or a divalent substituted hydrocarbon group; and m is 1 or 0).
Specific examples and preferable groups for R1 in the above-mentioned formulae (VI) to (XI) are the same as those in the above-mentioned formula (I).
Unsubstituted hydrocarbon groups as R7 and R8 in the above-mentioned formula (X) are preferably alkyl groups with 1 to 30 (more preferably 1 to 20) carbon atoms, aralkyl groups with 7 to 30 (more preferably 7 to 20) carbon atoms, or aryl groups with 6 to 30 (more preferably 6 to 20) carbon atoms when the two R7s and the two R8s do not from rings. Specifically, examples of the hydrocarbon group include methyl group, ethyl group, n-propyl group, iso-propyl group, n-butyl group, iso-butyl group, t-butyl group, pentyl group, cyclopentyl group, hexyl group, cyclohexyl group, octyl group, decyl group, dodecyl group, pentadecyl group, octadecyl group, benzyl group, 2-phenylethyl group, 1-phenylethyl group, phenyl group, 4-methylphenyl group, 1-naphthyl group, and 2-naphthyl group. When the two R7s and the two R8s form rings, five- to seven-membered rings are preferable, and more preferably, the two R7s and the two R8s may form rings composed of xe2x80x94(CH2)3xe2x80x94 group, xe2x80x94(CH2)4xe2x80x94 group, and/or xe2x80x94CHxe2x95x90CHxe2x80x94CHxe2x95x90CHxe2x80x94 group.
Substituted hydrocarbon groups as R7 and R8 in the above-mentioned formula (X) are preferably alkyl groups with 1 to 30 (more preferably 1 to 20) carbon atoms, aralkyl groups with 7 to 30 (more preferably 7 to 20) carbon atoms, or aryl groups with 6 to 30 (more preferably 6 to 20) carbon atoms, which are substituted with a substituent such as a halogen atom, an alkoxy group, a disubstituted amino group, or the like, when the two R7s and the two R8s do not from rings, and the specific examples include trifluoromethyl group, 2-t-butyloxyethyl group, 3-diphenylaminopropyl group, or the like. When the two R7s and the two R8s form a ring, the ring is preferably a five- to seven-membered ring which has the above-mentioned substituents, and more preferably the two R7s and the two R8s may form rings composed of xe2x80x94CH2xe2x80x94Oxe2x80x94CH2xe2x80x94 group, xe2x80x94(CH2)4xe2x80x94 group, and/or xe2x80x94CHxe2x95x90CHxe2x80x94CHxe2x95x90CHxe2x80x94 group, which has the above-mentioned substutuents.
As R7 and R8 in the above-mentioned formula (X), a hydrogen atom or a hydrocarbon group with 1 to 30 carbon atoms is preferred, and a hydrogen atom or an alkyl group with 1 to 20 carbon atoms is more preferred. Even more preferably, R7 is a hydrogen atom or an alkyl group with 1 to 20 carbon atoms and R8 is a hydrogen atom or methyl group.
Specific examples and preferable groups for R7 and R8 in the above-mentioned formula (XI) are the same as those in the above-mentioned formula (X).
The divalent unsubstituted hydrocarbon group as R9 in the above-mentioned formula (XI) is preferably an alkylene group with 1 to 30 (more preferably 1 to 20) carbon atoms, an aralkylene group with 7 to 30 (more preferably 7 to 20) carbon atoms, or an arylene group with 6 to 30 (more preferably 6 to 20) carbon atoms, and the specific examples include methylene group, 1,1-ethylene group, 1,2-ethylene group, 1,1-propylene group, 1,3-propylene group, 2,2-propylene group, 1,1-butylene group, 2,2-butylene group, 3-methyl-2,2-butylene group, 3,3-dimethyl-2,2-butylene group, 1,1-pentylene group, 3,3-pentylene group, 1,1-hexylene group, 1,1-heptylene group, 1,1-octylene group, 1,1-nonylne group, 1,1-dodecylene group, 1,1-pentadecylene group, 1,1-octadecylene group, 1,1-cyclopentylene group, 1,1-cyclohexylene group, phenylmethylene group, diphenylmethylene group, 1-phenyl-1,1-ethylene group, 9,9-fluorene group, xcex1,xcex1xe2x80x2-1,4-diisopropyl group, 1,2-phenylene group, 1,3-phenylene group, 1,4-phenylene group, or the like.
The divalent substituted hydrocarbon group as R9 in the above-mentioned formula (XI) is preferably an alkylene group with 1 to 30 (more preferably 1 to 20) carbon atoms, an aralkylene group with 7 to 30 (more preferably 7 to 20) carbon atoms, or an arylene group with 6 to 30 (more preferably 6 to 20) carbon atoms, and the specific examples include hexafluoro-2,2-propylene group, pentafluorophenylmethylene group, 4-methoxyphenylmethylene group, 4-dimethylaminophenylmethylene group, or the like.
As R9 in the above-mentioned formula (XI), an oxygen atom or a divalent hydrocarbon group is preferable, and an alkylene group with 1 to 20 carbon atoms or an aralkylene group with 7 to 20 carbon atoms is more preferable, and an alkylene group with 1 to 6 carbon atoms is even more preferable.
The content of the structures other than the repeating unit of the above-mentioned formula (I), which may be contained in the block structural unit represented by the formula (I), is preferably 20 units or less, more preferably 10 units or less, and even more preferably 5 units or less, based on 100 repeating units in the block structural units represented by the formula (I).
The unsubstituted arylene group as R2 in the above-mentioned formula (II) is preferably an arylene group with 6 to 30 (more preferably 6 to 20) carbon atoms, and the specific examples include 1,2-phenylene group, 1,3-phenylene group, 1,4-phenylene group, 2-methyl-1,4-phenylene group, 2,3-diemethyl-1,4-phenylene group, 2,5-diemethyl-1,4-phenylene group, 2,6-dimethyl-1,4-phenylene group, 2,3,5-trimethyl-1,4-phenylene group, tetramethyl-1,4-phenylene group, 2-ethyl-1,4-phenylene group, 2-propyl-1,4-phenylene group, 2-butyl-1,4-phenylene group, 2-pentyl-1,4-phenylene group, 2-hexyl-1,4-phenylene group, 2-phenyl-1,4-phenylene group, 2-benzyl-1,4-phenylene group, 1,4-naphthylene group, 2,3-naphthylene group, 1,5-naphthylene group, 2,6-naphthylene group, 4,4xe2x80x2-biphenylene group, 3,3xe2x80x2-biphenylene group, 3,4xe2x80x2-biphenylene group, 2,2xe2x80x2-biphenylene group, or the like.
The substituted allylene group as R2 in the above-mentioned formula (II) is preferably an arylene group with 6 to 30 (more preferably 6 to 20) carbon atoms which is substituted with a halogen atom, an alkoxy group, a disubstituted amino group, or the like, and the specific examples include tetrafluoro-1,4-phenylene group, 2-chloro-1,4-phenylene group, 2-ethoxy-1,4-phenylene group, 2-dimethylamino-1,4-phenylene group, or the like.
R2 in the above-mentioned formula (II) is preferably an arylene group with 6 to 20 carbon atoms, more preferably an arylene group with 6 to 12 carbon atoms, and even more preferably 1,4-phenylene group, 1,3-phenylene group, 2,5-dimethyl-1,4-phenylene group, or 2,6-naphthylene group.
The unsubstituted alkylene group as R3 in the above-mentioned formula (III) is preferably an alkylene group with 1 to 30 (more preferably 1 to 20) carbon atoms, and the specific examples include methylene group, 1,1-ethylene group, 1,2-ethylene group, 1,2-propylene group, 1,3-proypelene group, 1,4-butylene group, 1,5-penthylene group, 1,6-hexylene group, 1,12-dodecylene group, 1,18-octadecylene group, 1,4-cyclohexylene group, or the like.
The substituted alkylene group as R3 in the above-mentioned formula (III) is preferably an alkylene group with 1 to 30 (more preferably 1 to 20) carbon atoms which is substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific examples include chloro-1,2-ethylene group, tetrafluoro-1,2-ethylene group, methoxy-1,2-ethyelene group, methoxycarbonyl-1,2-ethylene group, or the like.
The unsubstituted aralkylene group as R3 in the above-mentioned formula (III) is preferably an aralkylene group with 7 to 30 (more preferably 7 to 20) carbon atoms, and the specific examples include 1-phenyl-1,1-methylene group, 2-phenyl-1,1-etheylene group, 1-phenyl-1,2-ethylene group, 1-phenyl-1,2-propylene group, 1,3-propylene group, 1-phenyl-1,4-butylene group, 1-phenyl-1,5-pentylene group, 1-phenyl-1,6-hexylene group, 1-phenyl-1,12-dodecylene group, or the like.
The substituted aralkylene group as R3 in the above-mentioned formula (III) is preferably an aralkylene group with 7 to 30 (more preferably 7 to 20) carbon atoms which is substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific examples include 4-chlorophenyl-1,2-ethylene group, 4-methoxyphenyl-1,2-ethylene group, or the like.
The unsubstituted alkenylene group as R3 in the above-mentioned formula (III) is preferably an alkenylene group with 2 to 30 (more preferably 2 to 20) carbon atoms, and the specific examples include 1,1-ethenylene group, 1,2-ethenylene group, 1,2-(1-propenylene) group, 1,3-(1-propenylene) group, 1,4-(1-butenylene) group, 1,5-(1-pentenylene) group, 1,6-(1-hexenylene) group, 1,12-(1-dodecenylene) group, 1,18-(1-octadecenylene) group, 1,4-(2-cyclohexenylene) group, or the like.
The substituted alkenylene group as R3 in the above-mentioned formula (III) is preferably an alkenylene group with 1 to 30 (more preferably 1 to 20) carbon atoms which is substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific examples include chloro-1,2-ethenylene group, tetrafluoro-1,2-ethenylene group, methoxy-1,2-ethenylene group, methoxycarbonyl-1,2-ethenylene group, or the like.
The unsubstituted aralkenylene group as R3 in the above-mentioned formula (III) is preferably an aralkenylene group with 8 to 30 (more preferably 8 to 20) carbon atoms, and the specific examples include 2-phenyl-1,1-ethenylene group, 1-phenyl-1,2-ethenylene group, 1-phenyl-1,2-(1-propenylene) group, 1,3-(1-propenylene) group, 1-phenyl-1,4-(1-butenylene) group, 1-phenyl-1,4-(2-butenylene) group, 1-phenyl-1,5-(1-pentenylene) group, 1-phenyl-1,6-(1-hexenylene) group, 1-phenyl-1,12-(1-dodecenylene) group, or the like.
The substituted aralkenylene group as R3 in the above-mentioned formula (III) is preferably an aralkenylene group with 8 to 30 (more preferably 8 to 20) carbon atoms which is substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific example include 4-chlorophenyl-1,2-ethenylene group, 4-methoxyphenyl-1,2-ethenylene group, or the like.
The unsubstituted alkynylene group as R3 in the above-mentioned formula (III) is preferably an alkynylene group with 2 to 30 (more preferably 2 to 20) carbon atoms, and the specific examples include ethenylene group, 1,3-(1-propynylene) group, 3,3-(1-propynylene) group, 1,4-(1-butynylene) group, 1,5-(1-pentynylene) group, 1,6-(1-hexynylene) group, 1,12-(1-dodecynylene) group, 1,18-(1-octadecynylene) group, or the like.
The substituted alkynylene group as R3 in the above-mentioned formula (III) is preferably an alkynylene group with 2 to 30 (more preferably 2 to 20) carbon atoms which is substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific examples include 3-chloro-1,3-(1-propynylene) group, 3,3-difluoro-1,3-(1-propynylene) group, or the like.
The unsubstituted aralkynylene group as R3 in the above-mentioned formula (III) is preferably an alkynylene group with 8 to 30 (more preferably 8 to 20) carbon atoms, and the specific examples include 3-phenyl-1,3-(1-propynylene) group, 3-phenyl-1,4-(1-butynylene) group, or the like.
The substituted aralkynylene group as R3 in the above-mentioned formula (III) is preferably an aralkynylene group with 8 to 30 (more preferably 8 to 20) carbon atoms which is substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific examples include 3-(4-chlorophenyl)-1,3-(1-propynylene) group, 3-(4-methoxyphenyl)-1,3-(1-propynylene) group, or the like.
R3 in the above-mentioned formula (III) is preferably an unsubstituted alkylene group with 1 to 30 carbon atoms, a substituted alkylene group with 1 to 30 carbon atoms, an aralkylene group with 7 to 30 carbon atoms, or an alkenylene group with 2 to 30 carbon atoms, and is more preferably an alkylene group with 1 to 25 carbon atoms or an alkenylene group with 2 to 20 carbon atoms, and is even more preferably an alkylene group with 1 to 20 carbon atoms or an alkenylene group with 2 to 10 carbon atoms.
T in the above-mentioned formulae (II) and (III) is xe2x80x94COxe2x80x94, xe2x80x94CONHxe2x80x94, or xe2x80x94SO2xe2x80x94, preferably xe2x80x94COxe2x80x94or xe2x80x94CONHxe2x80x94, and more preferably xe2x80x94COxe2x80x94.
Q in the above-mentioned formulae (II) and (III) is xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94SO2xe2x80x94, xe2x80x94OCOxe2x80x94, xe2x80x94NHCOxe2x80x94, or xe2x80x94OSi(CH3)2xe2x80x94, preferably xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94OCOxe2x80x94, xe2x80x94NHCOxe2x80x94, or xe2x80x94OSi(CH3)2xe2x80x94, more preferably xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, or xe2x80x94NHCOxe2x80x94, and even more preferably xe2x80x94Oxe2x80x94 or xe2x80x94COxe2x80x94.
The symbols b, c, d, and e in the above-mentioned formulae (II) and (III) are each 1 or 0, and at least one of c, d, and e is 1. The symbol b is preferably 1. The symbols d and e are each preferably 1.
The block copolymer in the present invention contains one or more block structural units represented by the formula (I) and one or more structural units represented by the formula (II) and/or the formula (III) in a molecule. The content of the block structural unit represented by the above-mentioned formula (I) is preferably 1 to 1,000 units, more preferably 1 to 100 units, and even more preferably 1 to 50 units in a molecule in the block copolymer in the present invention. The content of the structural units represented by the formula (II) and/or formula (III) is preferably 1 to 100,000 units, more preferably 1 to 10,000 units, and even more preferably 1 to 1,000 units in a molecule. Moreover, the block copolymer may contain two or more types of block structural units represented by the formula (I) and each two or more types of structural units represented by the formula (II) and/or formula (III).
The block copolymer in the present invention may be used as a mixture with a polymer having structural units represented by the above-mentioned formula (I) or with a polymer represented by the above-mentioned formula (II) and/or formula (III).
(2) Graft Polymer
The (2,5-disubstituted-1,4-phenylene oxide) graft polymer according to the present invention means a polymer which comprises one or more structural units represented by the formula (IV), or three or more of structural unit of the formula (IV) and structural unit of the formula (V), in a molecule.
The above-mentioned formula (IV) has the structural unit represented by the above-mentioned formula (I), and the specific and preferable examples of R1 and a in this structural unit are the same as those in the above-mentioned formula (I).
The trifunctional unsubstituted hydrocarbon group as R4 in the above-mentioned formula (IV) is preferably a trifunctional group with 1 to 30 (more preferably 1 to 20) carbon atoms and the specific examples include groups such 
The trifunctional substituted hydrocarbon group as R4 in the above-mentioned formula (IV) is preferably a trifunctional group with 1 to 30 (more preferably 1 to 20) carbon atoms substituted with a halogen atom, a hydroxyl group, an alkoxy group, a phenoxy group, an amino group, a substituted amino group, an alkoxycarbonyl group, an aminocarbonyl group, a nitrile group, or the like, and the specific examples include groups such as 
R4 in the above-mentioned formula (IV) is preferably a trifunctional hydrocarbon group, more preferably groups such as 
and even more preferably groups such as 
U in the above-mentioned formula (IV) is xe2x80x94COxe2x80x94, xe2x80x94OCOxe2x80x94, or xe2x80x94NHCOxe2x80x94, preferably xe2x80x94COxe2x80x94 or xe2x80x94NHCOxe2x80x94, and more preferably xe2x80x94COxe2x80x94. The symbol f is 1 or 0, preferably 1.
Specific and preferable examples of R5 in the above-mentioned formula (V) are the same as those of R4 in the above-mentioned formula (IV).
The halogen atom as R6 in the above-mentioned formula (V) represents a fluorine atom, a chlorine atom, a bromine atom, or an iodine atom, and among them, a fluorine atom or a chlorine atom is preferable.
Specific and preferable examples of the unsubstituted hydrocarbon group and substituted hydrocarbon group in the above-mentioned formula (V) are the same as those of R8 in the above-mentioned formula (XI).
W in the above-mentioned formula (V) represents xe2x80x94Oxe2x80x94, xe2x80x94COxe2x80x94, xe2x80x94CO2xe2x80x94, xe2x80x94OCOxe2x80x94, or xe2x80x94CONHxe2x80x94, preferably xe2x80x94Oxe2x80x94, xe2x80x94CO2xe2x80x94, or xe2x80x94CONHxe2x80x94, more preferably xe2x80x94Oxe2x80x94 or xe2x80x94CO2xe2x80x94, and even more preferably xe2x80x94CO2xe2x80x94.
The graft polymer in the present invention comprises one or more structural units represented by the formula (IV), or three or more of structural unit of the formula (IV) and structural unit of the formula (V), in a molecule. The content of the structural units represented by the formula (IV) is preferably 1 to 100,000 units, more preferably 1 to 10,000 units, even more preferably 1 to 1,000 units, and especially preferably 1 to 100 units, in a molecule. The content of the structural units represented by the formula (IV) and/or the formula (V) is preferably 3 to 1,000,000 units, more preferably 1 to 100,000 units, even more preferably 1 to 10,000 units, and especially preferably 1 to 1,000 units, in a molecule. The graft polymer may contain two or more types of structural units represented by the above-mentioned formula (IV) and may contain two or more types of structural units represented by the above-mentioned formula (V), in a molecule.
The graft polymer in the present invention may be used as a mixture with a polymer having structural units represented by the above-mentioned formula (I) or with a polymer represented by the above-mentioned formula (V), and furthermore, may be used as a mixture with the block copolymer of the present invention or with a polymer represented by the above-mentioned formula (II) and/or the formula (III).
Although no specific limitation is imposed on the shape of the polymer of the present invention, the polymer is preferably a powder with an average particle diameter of 5 mm or less and is more preferably a powder with an average particle diameter of 2 mm or less.
Although no specific limitation is imposed on the crystallinity of the polymer of the present invention, the polymer preferably shows an exothermic peak (crystallization peak) of 5 J/g or more at 150xc2x0 C. or more when cooled after being melted, and/or shows an endothermic peak (crystalline melting peak) of 5 J/g or more at 150xc2x0 C. or more when re-heated after the melted polymer is cooled.
The crystallization peak and crystalline melting peak of the polymer are measured as follows. In differential scanning calorimetry carried out under argon atmosphere, the polymer is heated from room temperature to a temperature at which it completely melts (complete melting temperature) at a rate of 10xc2x0 C./min, kept at the complete melting temperature for 5 minutes, cooled from the complete melting temperature to room temperature at a rate of 10xc2x0 C./min to check whether an exothermic peak (crystallization peak) of 5 J/g or more is present at 150xc2x0 C. or more. Subsequently, the polymer is heated again from room temperature to the complete melting temperature at a rate of 10xc2x0 C./min to check whether an endothermic peak (crystalline melting peak) of 5 J/g or more is present at 150xc2x0 C. or more.
The crystallization peak temperature of the polymer when cooled after melting is preferably 180xc2x0 C. or more, more preferably 200xc2x0 C. or more, and even more preferably 220xc2x0 C. or more. The quantity of heat for crystallization peak is preferably 6 J/g or more, more preferably 7 J/g or more, and even more preferably 10 J/g or more.
The melting peak temperature of the polymer when re-heated after melting and cooling of the polymer is preferably 200xc2x0 C. or more, more preferably 240xc2x0 C. or more, and even more preferably 270xc2x0 C. or more. The quantity of heat for melting peak is preferably 6 J/g or more, more preferably 7 J/g or more, and even more preferably 10 J/g or more.
More preferably, the polymer of the present invention is substantially free from gel substance. The polymer is confirmed to be free from gel substance, for example, when 1 mg of the polymer is dissolved in 1 ml of 1,2-dichlorobenzene at 150xc2x0 C. xe2x80x9cSubstantially free from gel substancexe2x80x9d means that the polymer preferably contains 5% by weight or less, more preferably 2% by weight or less of gel substance, and the polymer most preferably contains no gel substance.
Although no specific limitation is imposed on the molecular weight of the polymer of the present invention, the number average weight is preferably 500 to 1,000,000, more preferably 1,000 to 200,000, and even more preferably 2,000 to 100,000.
(3) Preparation Method of Copolymers
Preparation methods of the block copolymer of the present invention will be described hereinafter.
Although no specific limitation is imposed on the preparation method of the block copolymer of the present invention, it is preferable to synthesize a polymer having block structural units represented by the formula (I) and then copolymerize the polymer with at least one of structural units represented by the formula (II) or the formula (III).
Although no specific limitation is imposed on the synthesis method of the polymer having block structural units represented by the formula (I), it is preferable to subject a 2,5-disubstituted phenol represented by the following formula (XII) to oxidative polymerization in the presence of a copper complex catalyst comprising a tridentate ligand having nitrogen atoms as coordinating atoms and a copper atom, and in the presence of oxygen. The catalyst and the reaction conditions may be used according to the method described in Japanese Patent Application No.2000-25621. 
(wherein R1 has the same meaning as that in the above-mentioned formula(I))
Specific examples and preferable groups of R1 in the above-mentioned formula (XII) are the same as those in the above-mentioned formula (I).
Preparation methods of the above-mentioned block structural unit (polymer) will be described hereinafter.
A tridentate ligand in a copper complex catalyst means a tridentate ligand whose coordinating atoms are nitrogen atoms. The ligand means a molecular or an ion that is bonded to a certain atom by coordination bond, as described in Kagakudaijiten (1st ed., Tokyo Kagaku Dojin, 1989). The atom directly involved in the bond is called a coordinating atom. The tridentate ligand is a ligand having three coordinating atoms.
No specific limitation is imposed on the tridentate ligand used in the above-mentioned copper complex catalyst, provided that the coordinating atoms are nitrogen atoms. Specific examples of such a tridentate ligand include diethylene triamine, bis(2-pyridylmethyl)amine, bis(2-pyridylethyl)amine, bis(2-imidazolylmethyl)amine, bis(2-oxazolylmethyl)amine, bis(2-thiazolylmethyl)amine, N-(2-pyridylmethylidene)-N-(2-pyridylmethyl)amine, 2,2xe2x80x2:6xe2x80x2,2xe2x80x3-terpyridine, 3-(2-pyridylmethylimino)-2-butanoneoxime, tris(2-pyridyl)methane, tris(2-imidazolyl)methane, tris(1-pyrazolyl)methane, tris(1-pyrazolyl)phosphate, tris(1-pyrazolyl)borate, 1,4,7-triazacyclononane, and derivatives thereof.
The valence of the copper atom in the copper complex catalyst is 0 to 3, preferably 1 or 2. In the copper complex catalyst, no specific limitation is imposed on the ratio of the tridentate ligand and the copper atom, but one or more copper atoms are preferable, one to three copper atoms are more preferable, and one copper atom is further preferable, per tridentate ligand, as a substantially formed complex.
The copper complex catalyst can be used in an arbitrary amount. In general, the copper complex catalyst is preferably used at 0.001 to 50 mol %, more preferably 0.01 to 10 mol %, calculated as the amount of copper to the phenolic starting material.
The oxidant in oxidative polymerization reaction in preparation of the block structural unit is generally oxygen, which may be a mixture with an inert gas or may be air. Oxygen is usually used in large excess above the equivalent, to the phenolic starting material. Oxidative polymerization can be conducted in the absence of a reaction solvent, but usually a solvent is preferably used.
No specific limitation is imposed on the reaction temperature in oxidative polymerization, provided that the reaction medium remains fluid. When no solvent is used, a temperature equal to or above the melting point of the phenolic starting material is necessary. The preferable temperature range is 0xc2x0 C. to 200xc2x0 C., more preferably 0xc2x0 C. to 150xc2x0 C., and even more preferably 0xc2x0 C. to 100xc2x0 C. The preferable reaction temperature is 10xc2x0 C. to 60xc2x0 C. in view of energy saving. The reaction time varies depending on the conditions such as the amount of the catalyst and the reaction temperature, but the reaction time is generally 1 hours or more, preferably 3 to 300 hours.
The polymer having block structural units represented by the formula (I) may be obtained by oxidative polymerization of a 2,5-disubstituted phenol represented by the above-mentioned formula (XII) which may be used alone, or in combination with one another, or as a mixture with a phenol represented by the following formula (XIII) and/or a bisphenol (XIV) represented by the following formula (XIV). 
(wherein R7 and R8 each have the same meanings as those in the above-mentioned formula (X), and R10 is a hydrogen atom, a phenoxy group, an unsubstituted hydrocarbon group, or a substituted hydrocarbon group.) 
(wherein R7 to R9 and m each have the same meanings as those in the above-mentioned formula (XI).)
Specific examples and preferable groups for R7 and R8 in the above-mentioned formula (XIII) are the same as those in the above-mentioned formula (X).
R10 in the above-mentioned formula (XIII) is preferably a hydrogen atom, a phenoxy group, or a hydrocarbon group with 1 to 20 carbon atoms, more preferably a hydrogen atom, a phenoxy group, or a hydrocarbon group with 1 to 6 carbon atoms, and even more preferably a hydrogen atom or a phenoxy group.
Specific examples and preferable groups for R7 to R9 in the above-mentioned formula (XIV) are the same as those in the above-mentioned formula (XI).
When a 2,5-disubstitutied phenol represented by the above-mentioned formula (XII) is used in combination with a phenol represented by the above-mentioned formula (XIII) and/or a bisphenol represented by the above-mentioned formula (XIV), the ratio of each component is appropriately determined, provided that the properties of the desired polymer is not impaired, but the combination ratio of the 2,5-disubstitutied phenol is preferably 80 mol % or more, more preferably 90 mol % or more, and even more preferably 95 mol % or more, based on the total phenol monomers.
When a 2,5-disubstitutied phenol represented by the above-mentioned formula (XII) and/or a phenol represented by the above-mentioned formula (XIII) are subjected to oxidative polymerization, the polymer having block structural units represented by the formula (I) generally has a hydroxyl group only at one terminal in its molecule. On the other hand, a 2,5-disubstitutied phenol represented by the above-mentioned formula (XII) and/or a phenol represented by the above-mentioned formula (XIII) are subjected to oxidative polymerization in combination with a bisphenol represented by the above-mentioned formula (XIV), the polymer having block structural units represented by the formula (I) has structural units represented by the above-mentioned formula (XI) and generally has hydroxyl groups at both terminals in its molecule.
When a polymer having block structural units represented by the formula (I) is reacted with a carbonyl compound represented by R11xe2x80x94COxe2x80x94R12 or a halogen compound represented by Xxe2x80x94R13xe2x80x94X (wherein R11 and R12 each represent a hydrogen atom, an unsubstituted hydrocarbon group, or a substituted hydrocarbon group; R13 represents a divalent unsubstituted-hydrocarbon group or a divalent substituted-hydrocarbon group; and X represents a halogen atom such as chlorine, bromine, and iodine; specific examples and preferable groups for R11 and R12 are the same as those for R8 in the above-mentioned formula (XI); specific examples and preferable groups for R13 are the same as those for R9 in the above-mentioned formula (XI) excluding an oxygen atom.), a polymer having xe2x80x94C(R11R12)xe2x80x94 and xe2x80x94R13xe2x80x94 linkages and generally having hydroxyl groups at both terminals in its molecule can be obtained. No specific limitation is imposed on the reaction conditions of this method, and 0.5 or more equivalents of the carbonyl compound and the halogen compound are reacted, to the polymer having block structural units represented by the formula (I).
In the production of the block copolymer of the present invention, no specific limitation is imposed on the method to copolymerize so that at least one of the structural units represented by the formula (II) or the formula (III) is incorporated, the following method is preferable.
The first embodiment of block copolymerization is a method, in which a polymer having block structural units represented by the formula (I) is reacted with a halogen compound, such as XCOxe2x80x94R2xe2x80x94Oxe2x80x94CH3, XCOxe2x80x94R2xe2x80x94COX, Xxe2x80x94R3xe2x80x94H, Xxe2x80x94R3xe2x80x94Oxe2x80x94CH3, XCOxe2x80x94R3xe2x80x94H, XCOxe2x80x94R3xe2x80x94Oxe2x80x94CH3, XCOxe2x80x94R3xe2x80x94COX, Xxe2x80x94O2Sxe2x80x94R2xe2x80x94SO2xe2x80x94X, Xxe2x80x94O2Sxe2x80x94R3xe2x80x94SO2xe2x80x94X, or Xxe2x80x94COxe2x80x94X; or a cyclic acid anhydride represented by the following structural formula (XV) or (XVI) (wherein R2 has the same meaning as that in the formula (II); R3 has the same meaning as that in the formula (III); and X represents a halogen atom such as chlorine, bromine, or iodine.). 
No specific limitation is imposed on the reaction conditions for reacting the above-mentioned halogen compound or cyclic acid anhydride, and halogen atoms in the halogen compound, or the cyclic acid anhydride may be reacted at an equimolar amount or more, to the amount of the polymer having block structural units represented by the formula (I). When the above-mentioned halogen compound or the cyclic acid anhydride is reacted in the presence of a base such as a tertiary amine, the halogen compound or the cyclic acid anhydride generally reacts with a terminal hydroxyl group of the polymer having block structural units represented by the formula (I). On the other hand, when reacting in the presence of a Lewis acid such as aluminum chloride, the halogen compound or the cyclic acid anhydride generally reacts with an aromatic group at one terminal of the polymer having block structural units represented by the formula (I).
The second embodiment for preparing a block copolymer is a method, in which the polymer having block structural units represented by the formula (I) is reacted with a carboxylic acid, such as HOxe2x80x94COxe2x80x94R2xe2x80x94Oxe2x80x94CH3, HOxe2x80x94COxe2x80x94R2xe2x80x94COxe2x80x94OH, HOxe2x80x94COxe2x80x94R3xe2x80x94H, HOxe2x80x94COxe2x80x94R3xe2x80x94Oxe2x80x94CH3, or HOxe2x80x94COxe2x80x94R3xe2x80x94COxe2x80x94OH, a carboxylate, such as Rxe2x80x94Oxe2x80x94COxe2x80x94R2xe2x80x94Oxe2x80x94CH3, Rxe2x80x94Oxe2x80x94COxe2x80x94R2xe2x80x94COxe2x80x94Oxe2x80x94R, Rxe2x80x94Oxe2x80x94COxe2x80x94R3xe2x80x94H, Rxe2x80x94Oxe2x80x94COxe2x80x94R3xe2x80x94Oxe2x80x94CH3, or Rxe2x80x94Oxe2x80x94COxe2x80x94R3xe2x80x94COxe2x80x94Oxe2x80x94R, or an isocyanate compound, such as OCNxe2x80x94R2xe2x80x94Oxe2x80x94CH3, OCNxe2x80x94R2xe2x80x94NCO, OCNxe2x80x94R3xe2x80x94H, OCNxe2x80x94R3xe2x80x94Oxe2x80x94CH3, or OCNxe2x80x94R3xe2x80x94NCO (wherein R2 has the same meaning as that in the formula (II), and R3 has the same meaning as that in the formula (III).). No specific limitation is imposed on the reaction conditions of this method, and the carboxylic acid compound, the carboxylate compound, or the isocyanate compound may be reacted at an equimolar amount or more, to the amount of the hydroxyl groups in the polymer having block structural units represented by the above-mentioned formula (I). The carboxylic acid compound, the carboxylate compound, or the isocyanate compound generally reacts with the terminal hydroxyl group of the polymer having block structural units represented by the formula (I).
The third embodiment for preparing a block copolymer is a method, in which an oxycarbonyl compound, such as YCOxe2x80x94R2xe2x80x94OZ or YCOxe2x80x94R3xe2x80x94OZ (wherein R2 has the same meaning as that in the formula (II); R3 has the same meaning as that in the formula (III); Y represents a hydroxyl group, or a halogen atom, such as chlorine, bromine, or iodine; and Z represents a hydrogen atom or a CH3COxe2x80x94 group.), a cyclic ester compound represented by the following structural formula (XVII), or a cyclic ether compound represented by the following structural formula (XVIII) is polymerized, in the presence of the polymer having block structural units represented by the above-mentioned formula (I). No specific limitation is imposed on the reaction conditions of this method, an excess molar amount of the oxycarbonyl compound, the cyclic ester compound, or the cyclic ether compound may be polymerized, to the hydroxyl groups of the polymer having block structural units represented by the above-mentioned formula (I).
A homopolymer of the oxycarbonyl compound, the cyclic ester compound, or the cyclic ether compound, and the polymer having block structural units represented by the above-mentioned formula (I) may be reacted, to obtain a corresponding block copolymer. 
(wherein R3 has the same meaning as that in the formula (III).)
In any of the above-mentioned three embodiments, the reaction temperature is preferably 30 to 350xc2x0 C., more preferably 60 to 150xc2x0 C., and the reaction time is preferably 0.1 hours to 500 hours, more preferably 1 hour to 48 hours. The reaction molar ratio can be appropriately determined according to the ratio of the polymer having block structural units represented by the formula (I) and the structural units represented by the formula (II) or (III) in the desired block copolymer.
Preparation methods of the graft polymer of the present invention will be described hereinafter.
No specific limitation is imposed on the preparation method of the graft polymer of the present invention, and the unsaturated bond parts in the block copolymer represented by the formula (XIX) may be polymerized or the block copolymer represented by the formula (XIX) may be copolymerized with a component represented by the formula (XX) to synthesize the graft polymer. 
(wherein R1, U, a and f are defined as in the formula (IV), and R6, W, and g are defined as in the formula (IV). R14 and R15 each represents an unsubstituted alkenyl group, a substituted alkenyl group, an unsubstituted aralkenyl group, a substituted aralkenyl group, an unsubstituted alkynyl group, a substituted alkynyl group, an unsubstituted aralkynyl group, or a substituted aralkynyl group.)
Specific examples and preferable examples of R1, U, a, and f in the above-mentioned formula (XIX) are the same as those in the formula (IV). Specific examples and preferable examples of R6, W, and g in the above-mentioned formula (XX) are the same as those in the formula (IV).
The unsubstituted alkenyl group, the substituted alkenyl group, the unsubstituted aralkenyl group, the substituted aralkenyl group, the unsubstituted alkynyl group, the substituted alkynyl group, the unsubstituted aralkynyl group, and the substituted aralkynyl group as R14 in the above-mentioned formula (XIX) and R15 in the above-mentioned formula (XX) are the same as those for R3 in the formula (III).
No specific limitation is imposed on the reaction conditions of the graft polymerization, and the reaction may be carried out in the presence of an appropriate radical initiator and a reaction solvent. The reaction temperature is preferably 30 to 350xc2x0 C., more preferably 60 to 150xc2x0 C., and the reaction time is preferably 0.1 to 500 hours, more preferably 1 hour to 48 hours. Moreover, the reaction mol ratio can be appropriately determined according to the ratio of the structural units represented by the formula (IV) and the formula (V) in the desired graft polymer.
The resin composition includes the above-mentioned block or graft polymer that may further contain an ordinary polymer that is not the block or graft polymer. The resin composition of this invention may be the graft polymer which comprises one or more structural units represented by the following formula (IV), or that comprising three or more structural units of the following formula (IV) and structural unit of the following formula (V), in a molecule. The resin composition is not particularly limited in this invention. In the resin composition, average value of number of structural unit represented by the formula (IV), per polymer molecule, is preferably 0.04 unit or more, more preferably 0.1 unit or more, particularly preferably 0.3 unit or more. The sum of number of the structural units represented by the formula (IV) or the formula (V) is preferably 10 units or more per molecule on average, though not particularly limited in this invention.
The block copolymer and graft polymer of the present invention may be used alone or as a composition with the block copolymer and the graft polymer. Specific examples of polymer components of the composition include a polymer having structural units represented by the above-mentioned formula (I), a polymer having structural units represented by the above-mentioned formula (II) and/or formula (III), a polymer having structural units represented by the above-mentioned formula (IV), a polymer having structural units represented by the above-mentioned formula (V); polyolefins such as a polyethylene, a polypropylene, a polystyrene, a polyvinyl chloride, a polymethyl methacrylate, a polyvinyl acetate, a polyacrylonitrile, and copolymers thereof; polyethers such as a polyoxymethylene, a polyphenylene oxide, a poly(2,6-dimethyl-1,4-phenylene oxide), and copolymers thereof; polyesters such as a polyethylene terephthalate, a polybutylene terephthalate, a poly(ethylene-2,6-dinaphthalate), a poly(4-oxybenzoate), a poly(2-oxy-6-naphthalate), and copolymers thereof; polyamides such as nylon 6 and nylon 66 (trade names); polycarbonates; polyphenylenesulfides; polysulfones; polyethersulfones; polyether etherketones; polyimides; polyetherimides and thermosetting polymers such as phenol resins, urea resins, melamine resins, and epoxy resins. Specific examples of reformers for the composition include stabilizers such as 2,6-di-t-butylphenol derivatives and 2,2,6,6-tetramethylpiperidine derivatives; flame retardants such as polyhalogenated compounds and phosphates; surfactants; and rheology modifiers.
The (2,5-disubstituted-1,4-phenylene oxide) block copolymer and the (2,5-disubstituted-1,4-phenylene oxide) graft polymer, of the present invention, can increase the molecular weight of poly(2,5-disubstituted-1,4-phenylene oxide). It is expected that these copolymers further improve mechanical strength and impact strength of molded articles produced therefrom and are useful as raw materials for injection molding and materials for use as film.